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We present a new method for measuring the spectral phase of ultrashort pulses that utilizes spectral shearing interferometry with zero delay. Unlike conventional spectral phase interferometry for direct electric-field reconstruction, which encodes phase as a sensitively calibrated fringe in the spectral domain, two-dimensional spectral shearing interferometry robustly encodes phase along a second dimension. This greatly reduces demands on the spectrometer and allows for complex phase spectra to be measured over extremely large bandwidths, potentially exceeding 1.5 octaves.

We present three Cr3+:Colquiriite lasers as low-cost alternatives to Ti:Sapphire laser technology. Single-mode laser diodes, which cost only $150 each, were used as pump sources. In cw operation, with approximately 520 mW of absorbed pump power, up to 257, 269 and 266 mW of output power and slope efficiencies of 53%, 62% and 54% were demonstrated for Cr:LiSAF, Cr:LiSGaF and Cr:LiCAF, respectively. Record cw tuning ranges from 782 to 1042 nm for Cr:LiSAF, 777 to 977 nm for Cr:LiSGaF, and 754 to 871 nm for Cr:LiCAF were demonstrated. In cw mode-locking experiments using semiconductor saturable absorber mirrors at 800 and 850 nm, Cr:Colquiriite lasers produced approximately 50-100 fs pulses with approximately 1-2.5 nJ pulse energies at approximately 100 MHz repetition rate. Electrical-to-optical conversion efficiencies of 8% in mode-locked operation and 12% in cw operation were achieved.

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Over the last decade, the control of atomic-scale electronic motion by optical fields strong enough to mitigate the atomic Coulomb potential has broken tremendous new ground with the advent of phase-controlled high-energy few-cycle pulse sources. Further investigation and control of these physical processes, including high-harmonic generation, ask for the capability of waveform shaping on sub-cycle time scales, which requires a fully phase-controlled multiple-octave-spanning spectrum. In this paper, we present a light source that enables sub-cycle waveform shaping with a two-octave-spanning spectrum and 15 µJ pulse energy based on coherent synthesis of pulses with different spectra, or wavelength multiplexing. The synthesized pulse has its shortest high-field transient lasting only 0.8 cycles (amplitude FWHM) of the centroid frequency. The benefit of the approach lies in its modular design and scalability in both bandwidth and pulse energy. Full phase control allows for the synthesis of any optical waveform supported by the amplified spectrum. A numerical study shows the uniqueness of the light source for direct isolated soft-x-ray pulse generation based on high-harmonic generation, greatly reducing and eventually even eliminating the need for gating techniques or spectral filtering. The demonstrated system is the prototype of a class of novel optical tools for attosecond control of strong-field physics experiments.

Semiempirical molecular orbital theory and semiclassical solvent effect theory are used to analyze the conformational and electronic properties of the 12-s-cis and 12-s-trans conformers of 11-cis retinal. The goal is to examine the influence of solvent environment on the equilibrium geometries of these conformers as well as to provide a perspective on the electronic transitions that contribute to the four band systems that are observed in the 200-500 nm region of the optical spectrum. We conclude that the 12-s-cis isomer is more stable in vacuum, but that the 12-s-trans conformer is preferentially stabilized in both polar and nonpolar solvent environment due to dispersive as well as electrostatic interactions. This observation is in substantial agreement with previous literature results. In contrast, our analysis of the excited state manifold indicates that the spectral features observed in the absorption spectrum are associated with a complex set of overlapping transitions. A total of 18 pi*<--pi transitions contribute to the four bands, and in some cases, conformation changes the relative contribution of the individual transitions that define the overall band shape. This study provides the first definitive assignments for all four band systems.

Carrier-envelope phase stabilization of a 200MHz octave-spanning Ti:sapphire laser without external broadening is demonstrated. The individual comb lines spaced by 200MHz can conveniently be resolved using commercial wavemeters. The accumulated in-loop carrier-envelope phase error (integrated from 2.5 mHz to 10 MHz) using a broadband analog mixer as phase detector is 0.117 rad, equivalent to 50 attosecond carrier-envelope phase jitter at 800 nm.

Abstract:We demonstrate a tunable laser frequency comb operating near 420 nm with mode spacing of 20-50 GHz, usable bandwidth of 15 nm and output power per line of ~20 nW. Using the TRES spectrograph at the Fred Lawrence Whipple Observatory, we characterize this system to an accuracy below 1m/s, suitable for calibrating high-resolution astrophysical spectrographs used, e.g., in exoplanet studies.